Novel metal–organic frameworks (MOFs) based on thiabendazole (TBZ) were developed. The two structurally distinct TBZ-MOFs synthesized in this study exhibited enhanced durability and a broader biocidal spectrum than either individual bioactive species (i.e., Zn²⁺ and TBZ). The characteristics of each TBZ-MOF are related to the coordination modes among the Zn²⁺ ions and ligand donors. The difference in water solubility between the two TBZ-MOFs due to the structural design allows for the controlled release of the desired bioactive component.